Adiabatic climbing of vibrational ladders using Raman transitions with chirped pump lasers: effect of higher electronic surfaces and control of the shapes of vibrational wave packets
Bibliographic record
Abstract
Abstract Using numerical solutions of the time‐dependent Schrödinger equation for the H2 molecule in intense laser fields we calculate the vibrational excitation induced by the Raman chirped adiabatic process (RCAP). We show that adding several higher electronic surfaces to a simple two‐surface model improves the efficiency of the ladder‐climbing process at intensities below the adiabaticity threshold. Furthermore, we show that although using photon energies close to the one‐photon electronic transition frequency allows the use of lower pump and Stokes intensities, in general, this leads to more population transfer to the upper electronic surfaces accompanied by a loss of selectivity in the vibrational excitation on the ground‐state surface. By contrast, considerable dissociation yields can be achieved when higher energy photons are used. We also investigate the structure of time‐dependant vibrational wave packets prepared by RCAP. We find that at specific times the wave packet is very well localised at large inter‐nuclear separations at which ionisation occurs with a probability 3 orders of magnitude larger than at the equilibrium separation. Copyright © 2007 John Wiley & Sons, Ltd.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.001 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| Science and technology studies | 0.000 | 0.001 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.002 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one source (direct Gemma or distilled Codex), not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".